Nanjing University of Science & Technology

The hydrogen bonding network of tetramethylene sulfone (TMS)-water/heavy water binary solutions with different volume ratios was investigated using spontaneous and stimulated Raman spectra. The results indicate that, as the concentration of V_TMS increases, TMS does not engage in hydrogen bonding with water or heavy water. However, it influences the system by altering the molecular clustering of water and heavy water. In the mixed TMS-water binary solution, when the V_TMS is less than 60%, the addition of TMS leads to the transformation of the water molecules from a tetrahedral structure to dimers and trimers. In the TMS-heavy water binary solution, when the V_TMS is between 20% and 60%, the TMS leads to a change in the heavy water cluster structure by influencing the original force symmetry of the OD covalent bond, which causes the Raman peaks of OD symmetrical stretching vibration to shift to lower wavenumbers. When V_TMS is over 60%, the Raman peaks corresponding to the OH/D stretching vibration barely change due to the limited effect of excess TMS on the structure of water and heavy water clusters. When the V_TMS is over 25%, there is only one Raman peak in the stimulated Raman spectrum.

Esophageal cancer (EC) is one of the most prevalent malignant tumors globally, and the core strategy to improve the survival prospects of EC patients is to identify high-risk lesions and subsequently administer efficacious treatments. Among numerous biomarkers, microRNAs have the potential to facilitate rapid cancer screening and prevention. Therefore, a highly sensitive detection method based on photoinduced electron transfer atom transfer radical polymerization (PET-ATRP) signal amplification strategy was designed, aiming to accurately detect the potential markers of EC. The biosensor employs an indium tin oxide (ITO) electrode as a carrier, immobilizes probe 1 on the electrode surface by silanization, and achieves effective capture of tRNA with a stable sandwich structure to introduce -SH group. Subsequently, an ATRP initiator was introduced to the electrode surface by forming disulfide bonds, which resulted in the growth of poly-ferrocene under the catalysis of rhodamine 6G (R6G) and blue light irradiation. The R6G-mediated PET-ATRP signal amplification strategy offers significant advantages of simplicity, rapidity and cost-effectiveness while enhancing the sensitivity of the biosensor to tRNA with a limit of detection of 0.12 fM. Moreover, the biosensor exhibits excellent selectivity and anti-interference ability in real samples, which has significant potential for the timely prevention and diagnosis of EC.

This study innovatively integrates critical CO₂-assisted synthesis with defect engineering in two-dimensional materials to synergistically address the critical challenges of high overpotential and poor stability in acidic hydrogen evolution (HER) and oxygen evolution reactions (OER). Departing from conventional isolated studies on singular technologies or materials, we propose a novel defect-engineering strategy for polymetallic systems: By leveraging the unique physicochemical properties of critical-state CO₂, we precisely regulate the synergistic effects of dual defects (nitrogen doping and oxygen vacancies), achieving concurrent optimization of active sites and structural stability. Experimental results demonstrate that alloy catalysts synthesized under subcritical pressure exhibit excellent HER and OER performance (OER overpotential: 138.9 mV) and long-term stability under industrial-grade current densities. Through systematic comparison of materials synthesized under different CO₂ pressures, combined with mechanistic studies, we reveal the structure-activity relationship between CO₂-assisted synthesis and dual-defect (N-doping/O-vacancy) construction: The distinctive synthesis environment induced by critical pressure not only promotes uniform distribution of multimetallic elements but also optimizes the reaction pathway of the lattice oxygen mechanism (LOM) by modulating band structure and carrier concentration. This work provides a new paradigm for developing highly efficient and stable acidic HER/OER catalysts while demonstrating the universal applicability of critical-state synthesis technology in advanced alloy material fabrication.